Nonlinear Spectroscopy: Characterizing Fluctuations Andrei Tokmakoff MIT Department of Chemistry 2009.

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Presentation transcript:

Nonlinear Spectroscopy: Characterizing Fluctuations Andrei Tokmakoff MIT Department of Chemistry 2009

Fluctuations in lineshapes

System-Bath Interactions System: Spectroscopically Bright States Bath: Dark States → Energy Gap Fluctuations In spectroscopy … (Condon Approx.)

Energy Gap Fluctuations Energy Gap Correlation Function Dipole Correlation Function → Absorption lineshape Second Cumulant approx.

A bath of arbitrary form Spectral Density Brownian Oscillator Model

Nonlinear response for fluctuating system Following earlier approach: Cumulant approximation:

Two pulse echo ~1/ 

Two pulse echo

Lens analogy

Three pulse echoes: Peak shift

2D Lineshapes

Spectral Diffusion and Waiting Time

Time-domain 2D Spectroscopy

Time-Domain: Echo shape

2D IR Relaxation Experiment Probes Spectral Diffusion

Ellipticity

Correlation of Spectral Broadening

Correlation Effects in 2D IR Spectra

Correlated Energy Fluctuations Frequency Auto- and Cross-Correlation Functions:

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